Wadsworth Center, New York State Department of Health, Albany, New York 12201, United States; MOE Key Laboratory of Pollution Processes and Environmental Criteria, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China.
Wadsworth Center, New York State Department of Health, Albany, New York 12201, United States; School of Civil and Environmental Engineering, University of Science and Technology, Beijing 100083, China.
Environ Int. 2019 Jan;122:213-221. doi: 10.1016/j.envint.2018.11.007. Epub 2018 Nov 16.
Organophosphate esters (OPEs) are widely used as flame retardants and plasticizers in consumer products, which contributes to widespread exposure of humans. OPE diester metabolites in urine have been used as biomarkers of human exposure to these chemicals. Little is known, however, about occurrence and temporal variability in urinary concentrations of OPE metabolites in humans. In this study, 11 OPE metabolites were measured in 213 urine samples collected from 19 volunteers from Albany, New York, United States, at 3-day intervals for five weeks to investigate temporal variability in urinary concentrations. Diphenyl phosphate (DPHP) and bis(1,3-dichloro-2-propyl) phosphate (BDCIPP) were the major OPE metabolites, detected in all urine samples at specific gravity (SG)-adjusted concentrations (geometric mean, GM) of 1060 and 414 pg/mL and creatinine (Cr)-adjusted concentration (GM) of 404 and 156 ng/g, respectively. Inter-day variability in urinary OPE metabolite concentrations in 19 individuals was evaluated by intraclass correlation coefficients (ICCs). The inter-day variability in Cr-adjusted OPE metabolite concentrations (ICC: 0.31-0.67) was lower than those of SG-adjusted (ICC: 0.19-0.71) and unadjusted urinary concentrations (ICC: 0.24-0.74). BDCIPP (ICC: 0.68) and bis(2-chloroethyl) phosphate (BCEP) (ICC: 0.67) concentrations showed a moderate-to-high reliability over the sampling period, whereas the other nine OPE metabolites exhibited a moderate reliability (ICC: 0.31-0.55). Urine samples were further stratified by gender, age, ethnicity, and body mass index (BMI). The concentrations of BDCIPP and DPHP were significantly lower in males with normal BMI (BMI: 18.5-25 kg/m) than in females and other BMI categories (p < 0.01). Relatively high ICCs, indicating low inter-day variability, were observed for males (ICC: 0.35-0.71) of 30-40 years of age (ICC: 0.34-0.87) with normal BMI (ICC: 0.28-0.64). The daily exposure doses to OPEs were estimated from urinary concentrations of corresponding OPE metabolites. The estimated doses of triphenyl phosphate (TPHP) and triethyl phosphate (TEP), based on median urinary concentrations of their metabolites, were 19.4 and 24.0 ng/kg bw/day, and the exposure dose to ∑OPEs was estimated at 65.3 ng/kg bw/day. Overall, our results indicate a high ICC for Cr-adjusted urinary concentrations of 11 OPE metabolites in urine.
有机磷酸酯 (OPE) 广泛用作消费品中的阻燃剂和增塑剂，这导致人类广泛接触这些化学物质。尿液中的 OPE 二酯代谢物已被用作人体接触这些化学物质的生物标志物。然而，人们对人类尿液中 OPE 代谢物浓度的发生和时间变异性知之甚少。在这项研究中，我们在美国纽约奥尔巴尼的 19 名志愿者中采集了 213 份尿液样本，每隔 3 天采集一次，共采集 5 周，以研究尿液浓度的时间变异性。二苯基磷酸酯 (DPHP) 和双(1,3-二氯-2-丙基)磷酸酯 (BDCIPP) 是主要的 OPE 代谢物，在所有尿液样本中均以比重 (SG) 调整浓度 (几何均值，GM) 的 1060 和 414 pg/mL 和肌酐 (Cr) 调整浓度 (GM) 的 404 和 156 ng/g 检测到。通过内类相关系数 (ICC) 评估了 19 名个体尿液 OPE 代谢物浓度的日内变异性。Cr 调整的 OPE 代谢物浓度的日内变异性 (ICC：0.31-0.67) 低于 SG 调整的 (ICC：0.19-0.71) 和未调整的尿液浓度 (ICC：0.24-0.74)。BDCIPP (ICC：0.68) 和双(2-氯乙基)磷酸酯 (BCEP) (ICC：0.67) 浓度在整个采样期间具有中等到高度可靠性，而其他 9 种 OPE 代谢物则具有中度可靠性 (ICC：0.31-0.55)。根据性别、年龄、种族和体重指数 (BMI) 对尿液样本进行了进一步分层。正常 BMI (BMI：18.5-25 kg/m) 的男性尿液中的 BDCIPP 和 DPHP 浓度明显低于女性和其他 BMI 类别 (p < 0.01)。对于 30-40 岁的正常 BMI (BMI：18.5-25 kg/m) 的男性，观察到相对较高的 ICC (ICC：0.35-0.71)，表明日内变异性较低。)。根据相应 OPE 代谢物的尿液浓度，估算了 OPE 的每日暴露剂量。基于其代谢物的中位数尿液浓度，估算出三苯基磷酸酯 (TPHP) 和三乙基磷酸酯 (TEP) 的暴露剂量分别为 19.4 和 24.0 ng/kg bw/day，∑OPEs 的暴露剂量估计为 65.3 ng/kg bw/day。总体而言，我们的结果表明尿液中 11 种 OPE 代谢物的 Cr 调整尿液浓度具有较高的 ICC。
